I'm getting the set with From Russia With Love, Thunderball, and For Your Eyes Only, plus Dr. No as a single. I think we're pretty lucky to be getting 3 Connerys in the first batch of 6.
I first saw Bond in the theaters when Roger Moore was Bond, so those will always be some of my favorites. I've mostly experienced the Connery films with the advent of DVD, but I have found them to be more enduring and timeless than most of the last 10 or so Bond films. I liked Brosnan, but thought the scripts he had to work with usually started to bog down after an hour. Although I kind of like The Living Daylights, Dalton just doesn't do it for me. I saw an interview with him on one of the DVDs and could see why - he just had no presence or charisma, at least in my opinion. I love the reboot of the franchise and Casino Royale is my favorite of all. I thought the dialog was so much better in CR than any other Bond and I've rewatched it more in a year and a half than any other 007 movie.